@article{4bdf84713e1b4cdebb3f7ea7687526d9,
title = "Enhancing electrocatalytic N-2 reduction via tailoring the electric double layers",
abstract = "The electrocatalytic nitrogen reduction reaction (NRR) for NH3 synthesis is still far from being practical and competitive with the common Haber–Bosch process. The rational design of highly selective NRR electrocatalyst is therefore urgently needed, which requires a deep understanding of both the electrode–electrolyte interface and the mass transport of reactants. Here, we develop a theoretical framework that includes electric double layer (EDL), mass transport, and the NRR kinetics. This allows us to evaluate the roles of near-electrode environment and N2 diffusion on the NRR selectivity and activity. The EDL, as the immediate reaction environment, remarkably impedes the diffusion of N2 to the cathode surface at high electrode potentials, which explains experimental observations. This article also gives microscopic insights into the interplay between N2 diffusion and reaction activity under the nano-confinement, providing theoretical guidance for future design of advanced NRR electrocatalytic systems.",
keywords = "electric double layer, electrocatalytic N reduction, modified Poisson-Nernst-Planck equations, reaction-transport process",
author = "Haolan Tao and Cheng Lian and Hao Jiang and Chunzhong Li and Honglai Liu and {van Roij}, Rene",
note = "Funding Information: This work is part of the D-ITP consortium, a program of the Netherlands Organization for Scientific Research (NWO) that is funded by the Dutch Ministry of Education, Culture and Science (OCW). We acknowledge the EU-FET project NANOPHLOW (REP-766972-1). This work was also sponsored by the National Natural Science Foundation of China (No. 91834301, 22078088), the National Natural Science Foundation of China for Innovative Research Groups (No. 51621002), and the Shanghai Rising-Star Program (No. 21QA1401900). Funding Information: This work is part of the D‐ITP consortium, a program of the Netherlands Organization for Scientific Research (NWO) that is funded by the Dutch Ministry of Education, Culture and Science (OCW). We acknowledge the EU‐FET project NANOPHLOW (REP‐766972‐1). This work was also sponsored by the National Natural Science Foundation of China (No. 91834301, 22078088), the National Natural Science Foundation of China for Innovative Research Groups (No. 51621002), and the Shanghai Rising‐Star Program (No. 21QA1401900). Funding Information: EU‐FET project NANOPHLOW, Grant/Award Number: REP‐766972‐1; National Natural Science Foundation of China, Grant/Award Numbers: 91834301, 22078088, 51621002; Netherlands Organization for Scientific Research (NWO); Shanghai Rising‐Star Program, Grant/Award Number: 21QA1401900 Funding information Publisher Copyright: {\textcopyright} 2021 American Institute of Chemical Engineers.",
year = "2022",
month = mar,
doi = "10.1002/aic.17549",
language = "English",
volume = "68",
pages = "1--12",
journal = "AICHE Journal",
issn = "0001-1541",
publisher = "American Institute of Chemical Engineers",
number = "3",
}